Jahn-Teller distortion assisted interstitial nitrogen engineering:Enhanced oxygen dehydrogenation activity of N-doped Mn_(x)Co_(3-x)O_(4) hierarchical micro-nano particles  

作　　者：Yangxin Jin Fengfeng Li Peixin Cui Yun Yang Qingping Ke Minh Ngoc Ha Wangcheng Zhan Fei Ruan Chao Wan Zhao Lei Van Noi Nguyen Wei Chen Jun Tang 

机构地区：[1]College of Chemistry and Chemical Engineering Anhui University of Technology,Maanshan 243002,China [2]College of Chemistry and Materials Engineering Wenzhou University,Wenzhou 325035,China [3]Key Laboratory of Soil Environment and Pollution Remediation,Institute of Soil Science,Chinese Academy of Sciences,Nanjing 210008,China [4]VNU Key Laboratory of Advanced Material for Green Growth,VNU University of Science,Vietnam National University,Hanoi 100000,Vietnam [5]Key Laboratory for Advanced Materials and Research,Institute of Industrial Catalysis School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China

出　　处：《Nano Research》2021年第8期2637-2643,共7页纳米研究（英文版）

基　　金：supported by the Anhui Provincial Natural Science Foundation of China(2008085M47);“Key Program for International S&T Cooperation Projects of China”(No.2017YFE0124300);Anhui Provincial Science Fund for Excellent Young Scholars(gxyqZD2018034).

摘　　要：Rational design of earth-abundant transition metal oxides catalysts is highly desirable for developing sustainable chemical processes.Herein,we demonstrate a prospective interstitial nitrogen engineering for fabricating oxygen vacancies(OVs)-rich nitrogen-doped-Mn_(x)Co_(3-x)O_(4)(N-Mn_(x)Co_(3-x)O_(4))oxide catalyst,in which the ratio of OVs concentration of N-Mn_(x)Co_(3-x)O_(4)to Mn species is as high as 1:1,according to the characterizations of X-ray absorption(XAS)and X-ray photoelectron(XPS)spectroscopies.The promising strategy of interstitial nitrogen engineering through lattice distortion caused by the Jahn-Teller effect can significantly increase the amount of interstitial nitrogen.The resulting catalyst enables an additive-free aerobic dehydrogenation coupling of aromatic amine to afford azo compounds with>99%yield and>99%selectivity at 60☆.We observed the superb catalytic activity is promoted by the enhanced oxygen mobility in OVs,which were created by the interstitial nitrogen in the catalyst matrix.The presence of interstitial nitrogen in transition metal oxides in this study shows how the manipulation of catalyst matrix can increase the OV sites to promote aerobic oxidation reaction.

关 键 词：transition metal oxides Jahn-Teller effect interstitial nitrogen engineering MnxCo_(3-x)O_(4) DEHYDROGENATION 

分 类 号：O64[理学—物理化学]